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| 001 | 858791 | ||
| 005 | 20240610120404.0 | ||
| 024 | 7 | _ | |a 10.1021/jacs.8b01742 |2 doi |
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| 100 | 1 | _ | |a An, Jinghua |0 P:(DE-HGF)0 |b 0 |
| 245 | _ | _ | |a Acid-Promoter-Free Ethylene Methoxycarbonylation over Ru-Clusters/Ceria: The Catalysis of Interfacial Lewis Acid–Base Pair |
| 260 | _ | _ | |a Washington, DC |c 2018 |b American Chemical Society |
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| 520 | _ | _ | |a The interface of metal-oxide plays pivotal roles in catalytic reactions, but its catalytic function is still not clear. In this study, we report the high activity of nanostructured Ru/ceria (Ru-clusters/ceria) in the ethylene methoxycarbonylation (EMC) reaction in the absence of acid promoter. The catalyst offers 92% yield of MP with TOF of 8666 h–1, which is about 2.5 times of homogeneous Pd catalyst (∼3500 h–1). The interfacial Lewis acid–base pair [Ru-O-Ce-Vö], which consists of acidic Ce-Vö (oxygen vacancy) site and basic interfacial oxygen of Ru-O-Ce linkage, acts as active site for the dissociation of methanol and the subsequent transfer of hydrogen to the activated ethylene, which is the key step in acid-promoter-free EMC reaction. The combination of 1H MAS NMR, pyridine-IR and DFT calculations reveals the hydrogen species derived from methanol contains Brönsted acidity. The EMC reaction mechanism under acid-promoter-free condition over Ru-clusters/ceria catalyst is discussed. |
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| 700 | 1 | _ | |a Wang, Yehong |0 P:(DE-HGF)0 |b 1 |
| 700 | 1 | _ | |a Lu, Jianmin |0 0000-0003-3280-6466 |b 2 |
| 700 | 1 | _ | |a Zhang, Jian |0 P:(DE-HGF)0 |b 3 |
| 700 | 1 | _ | |a Zhang, Zhixin |0 0000-0003-1321-5273 |b 4 |
| 700 | 1 | _ | |a Xu, Shutao |0 P:(DE-HGF)0 |b 5 |
| 700 | 1 | _ | |a Liu, Xiaoyan |0 0000-0003-2694-2306 |b 6 |
| 700 | 1 | _ | |a Zhang, Tao |0 P:(DE-HGF)0 |b 7 |
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| 700 | 1 | _ | |a Heggen, Marc |0 P:(DE-Juel1)130695 |b 9 |
| 700 | 1 | _ | |a Dunin-Borkowski, Rafal |0 P:(DE-Juel1)144121 |b 10 |
| 700 | 1 | _ | |a Fornasiero, Paolo |0 0000-0003-1082-9157 |b 11 |
| 700 | 1 | _ | |a Wang, Feng |0 0000-0002-9167-8743 |b 12 |e Corresponding author |
| 773 | _ | _ | |a 10.1021/jacs.8b01742 |g Vol. 140, no. 11, p. 4172 - 4181 |0 PERI:(DE-600)1472210-0 |n 11 |p 4172 - 4181 |t Journal of the American Chemical Society |v 140 |y 2018 |x 1520-5126 |
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